Bridging the spatial gaps of the Ammonia Monitoring Network using satellite ammonia measurements.

Ammonia (NH) is a key precursor to fine particulate matter (PM) and a primary form of reactive nitrogen. The limited number of NH observations hinders further understanding of its impacts on air quality, climate, and biodiversity. Currently, NH ground monitoring networks are few and sparse across most of the globe, and even in the most established networks, large spatial gaps exist between sites and only a few sites have records that span longer than a decade. Satellite NH observations can be used to discern trends and fill spatial gaps in networks, but many factors influence the syntheses of the vastly different spatiotemporal scales between surface network and satellite measurements. To this end, we intercompared surface NH data from the Ammonia Monitoring Network (AMoN) and satellite NH total columns from the Infrared Atmospheric Sounding Interferometer (IASI) in the contiguous United States (CONUS) and then performed trend analyses using both datasets. We explored the sensitivity of correlations between the two datasets to factors such as satellite data availability and distribution over the surface measurement period as well as agreement within selected spatial and temporal windows. Given the short lifetime of atmospheric ammonia and consequently sharp gradients, smaller spatial windows show better agreement than larger ones except in areas of relatively uniform, low concentrations where large windows and more satellite measurements improve the signal-to-noise ratio. A critical factor in the comparison is having satellite measurements across most of the measurement period of the monitoring site. When IASI data are available for at least 80% days of AMoN's 2-week sampling period within a 25 km spatial window of a given site, IASI NH column concentrations and the AMoN NH surface concentrations have a correlation of 0.74, demonstrating the feasibility of using satellite NH columns to bridge the spatial gaps existing in the surface network NH concentrations. Both IASI and AMoN show increasing NH concentrations across CONUS (median: 6.8%·yr vs. 6.7%·yr) in the last decade (2008 - 2018), suggesting theNH will become a greater contributor to nitrogen deposition. NH trends at AMoN sites are correlated with IASI NH trends (r = 0.66), and show similar spatial patterns, with the highest increases in the Midwest and eastern U.S. In spring and summer, increases of NH were larger than 10%·yr in the eastern U.S. and Midwest (cropland dominated) and the western U.S. (pastureland dominated), respectively. NH hotpots (defined as regions where the IASI NH column is larger than the 95 percentile of 11-year CONUS map, 6.7 × 10 molec/cm), also experiencing increasing concentrations over time, with a median of NH trend of 4.7% · yr. IASI data show large NH increases in urban areas (8.1%·yr), including 8 of the top 10 most populous regions in the CONUS, where AMoN sites are sparse. A comparison between IASI NH concentration trends and state-level NH emission trends is then performed to reveal that positive correlations exist in states with strong agricultural NH emissions while negative correlations in states with low NH emissions and large NO emissions, suggesting the different roles of emission and partitioning in NH increases. The increases in NH could have detrimental effects on nearby eco-sensitive regions through nitrogen deposition and on aerosol chemistry in the densely populated urban areas, and therefore should be carefully monitored and studied.